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Aliphatic polyurethane (PU) nanocomposites were prepared using modified titanate nanotubes (TNTs) as filler in order to improve the mechanical and thermal properties of the initial polymer. With a view to achieving greater interaction between the polymer chains and TNTs, the latter was functionalized with hexamethylene diisocyanate (H) and/or aminopropyl trimethoxysilane groups (A), producing the modified nanotubes TNTH, TNTA, or TNTHA. The thermogravimetric analyses used to quantify the amount of anchored diisocyanate or/and silanol groups in the nanotubes identified the H function as the best functional group in terms of improving the filler–PU compatibility. Transmission electron microscopy, field emission scanning electron microscopy, and atomic force microscopy analyses of the PU nanocomposites containing the three different fillers showed good TNT dispersion. The TNTHA nanotubes functionalized with both groups through the reaction between the H function already anchored on the TNTs and the A group, forming a monourea anchored group, significantly improved the mechanical and thermal properties of PU nanocomposites. POLYM. COMPOS., 40:2292–2300, 2019. © 2018 Society of Plastics Engineers [ABSTRACT FROM AUTHOR]